ARTICLE Received 18 Jul 2013 | Accepted 7 Nov 2013 | Published 11 Dec 2013
DOI: 10.1038/ncomms3893
5d iridium oxide as a material for spin-current detection Kohei Fujiwara1,w, Yasuhiro Fukuma1,w, Jobu Matsuno1,w, Hiroshi Idzuchi2, Yasuhiro Niimi2, YoshiChika Otani1,2,w & Hidenori Takagi1,3
Devices based on pure spin currents have been attracting increasing attention as key ingredients for low-dissipation electronics. To integrate such spintronics devices into chargebased technologies, electric detection of spin currents is essential. The inverse spin Hall effect converts a spin current into an electric voltage through spin-orbit coupling. Noble metals such as Pt and Pd, and also Cu-based alloys, have been regarded as potential materials for a spincurrent injector, owing to the large direct spin Hall effect. Their spin Hall resistivity rSH, representing the performance as a detector, is not large enough, however, due mainly because of their low charge resistivity. Here we report that a binary 5d transition metal oxide, iridium oxide, overcomes the limitations encountered in noble metals and Cu-based alloys and shows a very large rSHB38 mO cm at room temperature.
1 RIKEN
Advanced Science Institute, Wako, Saitama 351-0198, Japan. 2 Institute for Solid State Physics, University of Tokyo, Kashiwa, Chiba 277-8581, Japan. of Physics, University of Tokyo, Hongo, Tokyo 113-0033, Japan. w Present addresses: The Institute of Scientific and Industrial Research, Osaka University, Ibaraki, Osaka 567-0047, Japan. (K.F.); Frontier Research Academy for Young Researchers, Kyushu Institute of Technology, Iizuka, Fukuoka 820-8502, Japan. (Y.F.); RIKEN Center for Emergent Matter Science (CEMS), Wako, Saitama 351-0198, Japan. (J.M., Y.O.). Correspondence and requests for materials should be addressed to K.F. (email: [email protected]). 3 Department
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NATURE COMMUNICATIONS | DOI: 10.1038/ncomms3893
S
pin-orbit coupling (SOC) is a relativistic effect and relates the spin moment of an electron to its orbital momentum via a momentum-dependent effective magnetic field. In the presence of SOC, a charge current without any spin polarization can be converted into a pure spin current (the flow of spin angular momentum) and vice versa, known as the direct spin Hall effect and the inverse spin Hall effect (ISHE)1–18. The presence of these phenomena in non-magnetic semiconductors had already been recognized in 1970s (refs 19–22) but recent theoretical1,2 and experimental investigations3,4 have given a boost to this field. Spin current-based electronics with low-energy consumption has since been discussed, where spin-current injection and detection, using charge/spin conversion by direct spin Hall effect and ISHE, played a key role. A variety of materials have subsequently been explored to realize efficient charge/spin conversion5–18. The playground for the exploration was first limited to semiconductors but then extended to metals, where we can take advantage of the less pronounced effect of interfacial barriers. Heavy transition metals such as Pt6–10,14, Au9,12,13, and Pd8,9,11 and also Cu-based alloys17,18 were found to exhibit a particularly large spin Hall angle aSH (the maximum yield of the charge/spin conversion), 0.01–0.1 at room temperature, owing to their pronounced SOC effects. These effects give these metals an advantage for application as a spin injector. In addition to the large aSH, their low electrical resistivity (rC), typically rC ¼ 10 7–10 5 O cm, allows large charge currents to be passed and hence to inject a large spin current without serious Joule heating. Spin currents can be detected by using the ISHE. In contrast to the case for spin injectors, the low rC of the heavy metals with a large aSH is a disadvantages when it comes to spin detection. In the ISHE, the electric voltage DVISHE generated by a spin current IS is in proportion to rC (refs 23,24): DVISHE / aSH rC IS rSH IS :
ð1Þ
Spin Hall resistivity given by rSH aSH rC determines the efficiency of spin-current detection. This means that a sensitive detection of spin current could be achieved in materials with both a large aSH and a high rC. In typical heavy metals, their low rC imposes strong constraints in tuning the value of rSH as it remains as low as o1 mO cm. One of the obvious approaches to improve the performance of spin detectors could be to increase the rC by alloying. Alloying can in fact increase not only the rC but also the aSH through an extrinsic spin Hall effect25–27. At room temperature where the inelastic scattering of charge carriers is dominant, however, it should be hard to anticipate a drastic increase of rC by alloying, for example, more than an order of magnitude increase as compared with the pristine material. Therefore, the improvement of rSH would not be achieved only by alloying. In this work, we propose 5d transition metal oxides (TMOs) as alternative metals to realize both large aSH and large rC, which should enhance rSH. The uniqueness of 5d TMOs is characterized by the extremely strong SOCB0.5–1 eV originating from the predominant 5d character of the conduction band. The SOC in 5d TMOs is in fact as strong as to reconstruct the electronic structures drastically, as first discussed in the case of Jeff ¼ 1/2 Mott state Sr2IrO4 (ref. 28). The analogous predominant SOC effect has been commonly observed in a broad range of Ir oxides including Ba2IrO4 (ref. 29), CaIrO3 (ref. 30) and Ir2O4 (ref. 31). In those Ir oxides, in addition to the strong SOC, the localized character of d orbitals gives rise to a moderately high charge resistivity rC even in the metallic state. Typical rC values of conductive 5d Ir TMOs such as IrO2 and SrIrO3 at room temperature are of the order of 10 4–10 3 O cm, at least one order of magnitude higher than those of normal s metals. As the variety of materials continues to grow rapidly, 5d TMOs offer a 2
unique opportunity to explore the giant rSH for efficient spin detection. We selected a simple binary oxide, rutile IrO2 (refs 32–34), as the basis for our exploration. IrO2 with Ir4 þ shares the same 5d5 configuration with many other Ir oxides, where the strong SOC dominates the electronic states and the resultant electronic properties34. This binary oxide has been long used as an electrode in various device applications, ranging from non-volatile ferroelectric memories to electrochemical devices. The excellent electrode properties are due to the formation of a clean, well-defined interface with other materials owing to its high chemical and thermal stability, and superior barrier properties for oxygen diffusion. In such a clean interface, it may be possible to inject a spin current through a diffusion process; IrO2 is therefore an ideal platform for testing the ISHE of 5d TMOs. Here, we describe successful spin-current injection into IrO2 using a lateral spin-valve (LSV) device geometry and demonstrate the ISHE with a remarkably high rSH as a metal not only in the polycrystalline state but also in the practically important amorphous state. Results Device structure. We fabricated cross-junction-type devices consisting of an IrO2 wire and a permalloy(Ni80Fe20, Py)/Ag/Py LSV35, shown in Fig. 1a,b (see also Methods). Spin currents are passed in the Ag strip by a non-local charge current injection (IC) from the ferromagnetic Py electrode and are perpendicularly injected in part into the IrO2 wire through the diffusion (Fig. 1a). This effect, called spin absorption, enables us to conduct a quantitative analysis of the ISHE as have been demonstrated for various materials7,8,17,18. We examined the potential of polycrystalline and amorphous IrO2 wires as the spin detector element. Their resistivities were 2.0 10 4 O cm and 5.7 10 4 O cm at 300 K, respectively, which are 1–2 orders of magnitude higher than those of metals that have been studied to date as a spin Hall material.
H
V
IC Ag Py1 Py2
IrO2
IrO2 Py1
Py2
Ag
Figure 1 | Inverse spin Hall effect measurements using a spin absorption effect in a lateral spin-valve geometry. (a) The structure of device used for ISHE measurements is shown schematically. A LSV with two Py electrodes (Py1: spin source, Py2: spin detector) bridged by an Ag spin transport layer was formed on an IrO2 wire. Spin-polarized charge current, IC, was injected along the arrow to accumulate pure spin currents in the Ag. The diffusion of spin current into the IrO2 wire, namely, the spin absorption, gives rise to the ISHE in IrO2. (b) Scanning electron microscopy image of a typical device. Scale bar, 500 nm. The dotted lines indicate the side edges of the IrO2 wire for clarity.
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NATURE COMMUNICATIONS | DOI: 10.1038/ncomms3893
To check that the Ag layer is not oxidized by directly contacting with IrO2, we first characterized the Ag/IrO2 interface by means of interface resistance measurements36. The current– voltage characteristics of the Ag/IrO2 interface showed an ohmic behaviour, typical of metal/metal interface. The slope of the data yielded a resistance–area product (RA) of 2.3 fO m2 at 300 K, which is as low as that of the metallic, transparent Ag/Py interface (RA ¼ 1.9 fO m2 at 300 K). An estimate of the thickness of the possibly oxidized Ag layer, using the resistivities of Ag2O and AgO in the literature37, never exceeded 0.1 nm. These observations imply that the Ag/IrO2 interface in the present devices is very sharp as in metal/metal interfaces. Spin-current injection into IrO2. The spin absorption by IrO2 across the interface was then confirmed by non-local spin-valve (NLSV) experiments7,8,17,18,35. The schematic diagram of the measurement is shown in Fig. 2a. The pure spin currents accumulated in the Ag strip by injecting spin-polarized charge currents IC from Py1 to Ag is detected as a voltage VS ( ¼ V þ V ) between Py2 (V þ ) and Ag (V ) (upper panel). The spin accumulation signal DRS is given by the difference in VS/ IC (RS) between parallel (high RS) and antiparallel (low RS) magnetizations of the two Py wires. If an IrO2 middle wire is in contact with the Ag, the accumulated spin diffuses in part into it (lower panel), resulting in the reduction in DRS (ref. 7). Figure 2b and c show field dependences of RS at 300 and 10 K, respectively. The decrease of DRS by the insertion of the IrO2 middle wire indicates the spin absorption effect. This is more clearly demonstrated in the temperature (T) dependence of DRS with (DRwith ) and without (DRwithout ) the middle wire, as S S is displayed in Fig. 2d. At all the temperatures, DRwith S , while both are enhanced systematically smaller than DRwithout S
at low temperatures owing to the increase of the spin-diffusion length of Ag (lAg)35. By analysing the data based on the threedimensional spin-diffusion model18 (see Supplementary Methods and Supplementary Fig. S1), we estimated a spin-diffusion length in polycrystalline IrO2, lIrO2 ¼ 3.8 nm at 300 K and 8.4 nm at 10 K, which are comparable to those of Pt (3–10 nm at 300 K (refs 6–10,14)) and CuIr (5–20 nm at 10 K (ref. 17)) where relatively large spin Hall angles were observed. This indicates that spin scattering of IrO2 is indeed very strong as expected from the 5d conduction band34. ISHE and qSH of IrO2. By injecting spin currents through the spin absorption effect, we successfully observed ISHE in IrO2. In Fig. 3a,b, we plot the room-temperature ISHE signal RISHE (DVISHE/IC) for polycrystalline and amorphous samples as a function of the magnetic field (The temperature dependence of the ISHE is shown in Supplementary Fig. S2 and is explained in Supplementary Note 1). Here the magnetic field was applied along the hard axis of the Py spin source (see Fig. 1a), and DVISHE was induced along the long-axis direction of the IrO2 wire. Reflecting the magnetization process in hard axis of Py, RISHE linearly increased up to B1,500 Oe and then saturated. The antisymmetric response to the applied magnetic field excludes any spurious effects such as anisotropic magnetoresistance of Py; the ISHE of IrO2 is responsible for the resistance change (2DRISHE) between positive and negative magnetic fields. The in-plane angular dependence of magnetic field effect on RISHE was confirmed fully consistent with the ISHE origin. Figure 3c shows the variation in RISHE under a magnetic field direction rotated by f with respect to the ordinary set-up (Fig. 3d, inset). The sign change of RISHE occurs between f ¼ 0 and p by magnetization switching of Py and concomitant polarization reversal of the spin
Without IrO2
RS (mΩ)
0
VS
H
V
IC
–0.2 –0.4 –0.6
Ag
Py2 With IrO2 H
300 K 10 K
0
RS (mΩ)
Py1
w/o IrO2 w/IrO2
–0.5 –1.0 –1.5
VS V
–2.0 –400 –200 0 200 400 H (Oe)
IC
IrO2
ΔRS (mΩ)
1.5 w/o IrO2
1.0 0.5 w/IrO2 0 0
100 200 T (K)
300
Figure 2 | Non-local spin-valve measurements. (a) The set-up of measurement is schematically depicted. The magnetic field H is applied along the easy axis of the Py electrodes. (b,c) NLSV signals measured at 300 K and 10 K for Py/Ag/Py LSVs without and with the polycrystalline IrO2 middle wire. (d) Temperature dependences of the NLSV signals. NATURE COMMUNICATIONS | 4:2893 | DOI: 10.1038/ncomms3893 | www.nature.com/naturecommunications
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IrO2 Polycrystalline w = 170 nm
RISHE (mΩ)
RISHE (mΩ)
0.2 0.1
2ΔRISHE
0
=0
0 =π
–0.2 –4,000
–0.1
0 H (Oe)
4,000
0.2
2ΔRISHE (mΩ)
RISHE (mΩ)
0.1
Amorphous w = 100 nm w = 170 nm
0
0.1 0 H
–0.1
–0.1
–0.2 –4,000 –2,000
0 H (Oe)
2,000
4,000
0
π/2 (rad)
π
Figure 3 | Inverse spin Hall effect of IrO2 at 300 K. (a) The ISHE signal RISHE (DVISHE/IC) for a polycrystalline IrO2 wire with a width w of 170 nm was measured as a function of the applied magnetic field H. (b) The results for amorphous IrO2 samples. Two devices with different w values (100 and 170 nm) were measured. The 100 nm-width device showed larger RISHE because of the increase of spin-current density. RISHE of the two amorphous devices are smaller than that of the polycrystalline sample shown in a. (c,d) Angular dependence of RISHE and the resistance change 2DRISHE by the ISHE. The in-plane azimuthal angle f with respect to the long axis of Ag is rotated to change the polarization direction of the spin current (inset in d). The solid line in d is a cos f curve fitted to the results.
current. As shown in Fig. 3d, the resistance change 2DRISHE vanishes at f ¼ p/2 and exhibits a cos f relation. This characteristic angular dependence is the hallmark of ISHE7,12, evidencing spin-dependent electron scattering in IrO2. Because of the large difference in rC between Ag and IrO2, the charge current induced in the IrO2 wire by the ISHE is partially shunted by the adjacent Ag layer. To take into account such geometric effects and to precisely determine rSH, we adopted the three-dimensional spin-diffusion model (see also Supplementary Methods). Using the ISHE signal 2DRISHE and data obtained from the NLSV measurements, aSH and rSH are, respectively, calculated to be 0.040 and 8.0 mO cm for polycrystalline IrO2, and 0.065 and 37.5 mO cm for amorphous IrO2 at 300 K. Figure 4 summarizes spin Hall resistivity rSH and electrical resistivity rC for a variety of metals with a large spin Hall angle aSH reported so far, together with that for IrO2. It mimics the point of this work in that rSH of IrO2 is distinctly large compared with typical heavy metals and their alloys of which rSH is B0.16–1.2 mO cm (refs 6–14,17,18), and is now comparable to the large rSH that was recently discovered in ultrathin films of b-phase (A15 crystal structure) W (ref. 15) and Ta (ref. 16). Discussion To generate a large electric voltage using the ISHE of IrO2 from existing metal-based spin-current devices, it is important to reduce the shunting effect at the Ag/IrO2 interface due to their large difference in rC. One of the promising approaches is to use Al (ref. 38) and Mg (ref. 39) as the non-magnetic spin transport layer. Their rC values are one order of magnitude higher than that of Ag we used, of the order of 10 mO cm at room temperature, while a comparably long spin-diffusion length is obtained. Another interesting route is a spin transport layer based on a conductive oxide composed of light elements with small 4
SOC. For example, in ZnO (ref. 40), doping with Al yields rC of the order of 100 mO cm (ref. 41), which can match with that of IrO2. The high chemical stability of IrO2 could be advantageous in fabricating such oxide-based junctions. The discovery of the ISHE in amorphous IrO2, which can be grown at room temperature, is a significant step towards spintronics devices based on such oxide materials. The comparably large aSH in the amorphous form may point to that spin scattering in this compound occurs at the length scale of as short as a unit cell, potentially enabling the spin detection at the atomic layer thickness. Although the physics of spin scattering in amorphous states has not been understood yet, the availability of the amorphous form should make it easier to study SOC-induced transport phenomena in 5d TMOs not used before in spintronics. In conclusion, 5d TMOs are the most promising materials for spin detection in spintronics. We demonstrated that the combination of strong SOC and a moderately high rC is a key to improve the performance of spin detection. These achievements in the simple binary oxide manifest the potential of 5d TMOs as a new class of spintronic materials. Strong SOC in this class of materials produces a rich variety of intriguing physical properties, including correlated topological insulator42, Weyl semi-metal43 and Kitaev spin liquid44. Our discovery of the large spin Hall resistivity may make 5d TMOs even more fascinating. Methods Device fabrication. The Py/Ag/Py LSV with an IrO2 middle wire was fabricated on a SiO2/Si substrate. Au/Ti leads for electrical measurements were prepared on the substrate by a photolithography and an e-beam deposition. IrO2 film was grown by a reactive sputtering with a 99.9% pure Ir target. A wire structure of IrO2 was formed using a posi-type resist patterned by an e-beam lithography. The typical wire width and thickness were 170 and 15 nm, respectively. During the deposition, the substrate was not heated, and the pressure was fixed at 0.7 Pa of Ar/O2 (90:10) mixture gas. X-ray diffraction analysis indicated that the as-deposited IrO2 film was amorphous. The amorphous film turned into
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V 10–4 -W15
a-IrO2
|SH| (Ω cm)
-Ta16 poly-IrO2
10–5
Pt14 CuIr17
CuBi18 10–6
Pt10 Pt9 Pd8
Au12 Pt8 SH=0.1 10–7 –6 10
10–5
Ta8 Nb8 Pd11 Mo8
SH=0.01 10–4 C (Ω cm)
10–3
Figure 4 | Spin Hall resistivity of metals. Experimentally measured values of spin Hall resistivity rSH for various metals are plotted as a function of electrical resistivity rC. Data include Pt (refs 9,10) and Pd (ref. 11) evaluated at room temperature by spin pumping, Pt (ref. 14) and atomic layer thin films of b-W (ref. 15) and b-Ta (ref. 16) at room temperature by spintransfer-torque ferromagnetic resonance, Au at 295 K using a planar Hall device12, Ta, Nb, Pd, Mo, Pt (ref. 8), 12% Ir-doped Cu (ref. 17), 0.5% Bidoped Cu (ref. 18) at 10 K, and polycrystalline and amorphous IrO2 at 300 K (this work) by spin absorption.
polycrystalline after a post-annealing at 400 °C in air. The LSV with a Py–Py separation of 700 nm (centre-to-centre) was then formed onto the IrO2 wire by the shadow evaporation method35,36. To prevent the surface oxidation of Ag, a 2-nmthick MgO protection layer was e-beam deposited on the surface without breaking vacuum. The width and thickness of wire were 170 and 100 nm for Ag, and 170 and 20 nm for Py, respectively. Their rC and spin-diffusion length were 3.0 mO cm and 330 nm for Ag and 47 mO cm and 5 nm for Py, respectively, at 300 K. One of the two Py electrodes was made longer than the other (not shown in Fig. 1b) to make the contrast in the fields for magnetization reversal. Electrical measurements. All electrical measurements were performed by a standard lock-in technique in a He flow cryostat. An alternating current IC of 200 mA with a frequency of 79 Hz was used for NLSV measurements. In ISHE measurements, IC of 400 mA was applied. We confirmed the linearity between the output voltage DVISHE and IC in the range of 100–400 mA.
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Acknowledgements
Additional information
We thank K. Ohgushi for helpful discussions. This work was supported by Grants-in-Aid (number 22340108, 23103518 and 24224010) from MEXT, Japan.
Supplementary Information accompanies this paper at http://www.nature.com/ naturecommunications Competing financial interests: The authors declare no competing financial interests.
Author contributions K.F., Y.F. and J.M. designed the experiments. K.F., Y.F. and H.I. fabricated devices and collected the data. K.F. and Y.N. analysed the data. K.F. wrote the manuscript with input from J.M. Y.O., and H.T. H.T. and Y.O. planned and supervised the project. All authors discussed the results.
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DOI: 10.1038/ncomms3893
5d iridium oxide as a material for spin-current detection Kohei Fujiwara1,w, Yasuhiro Fukuma1,w, Jobu Matsuno1,w, Hiroshi Idzuchi2, Yasuhiro Niimi2, YoshiChika Otani1,2,w & Hidenori Takagi1,3
Devices based on pure spin currents have been attracting increasing attention as key ingredients for low-dissipation electronics. To integrate such spintronics devices into chargebased technologies, electric detection of spin currents is essential. The inverse spin Hall effect converts a spin current into an electric voltage through spin-orbit coupling. Noble metals such as Pt and Pd, and also Cu-based alloys, have been regarded as potential materials for a spincurrent injector, owing to the large direct spin Hall effect. Their spin Hall resistivity rSH, representing the performance as a detector, is not large enough, however, due mainly because of their low charge resistivity. Here we report that a binary 5d transition metal oxide, iridium oxide, overcomes the limitations encountered in noble metals and Cu-based alloys and shows a very large rSHB38 mO cm at room temperature.
1 RIKEN
Advanced Science Institute, Wako, Saitama 351-0198, Japan. 2 Institute for Solid State Physics, University of Tokyo, Kashiwa, Chiba 277-8581, Japan. of Physics, University of Tokyo, Hongo, Tokyo 113-0033, Japan. w Present addresses: The Institute of Scientific and Industrial Research, Osaka University, Ibaraki, Osaka 567-0047, Japan. (K.F.); Frontier Research Academy for Young Researchers, Kyushu Institute of Technology, Iizuka, Fukuoka 820-8502, Japan. (Y.F.); RIKEN Center for Emergent Matter Science (CEMS), Wako, Saitama 351-0198, Japan. (J.M., Y.O.). Correspondence and requests for materials should be addressed to K.F. (email: [email protected]). 3 Department
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S
pin-orbit coupling (SOC) is a relativistic effect and relates the spin moment of an electron to its orbital momentum via a momentum-dependent effective magnetic field. In the presence of SOC, a charge current without any spin polarization can be converted into a pure spin current (the flow of spin angular momentum) and vice versa, known as the direct spin Hall effect and the inverse spin Hall effect (ISHE)1–18. The presence of these phenomena in non-magnetic semiconductors had already been recognized in 1970s (refs 19–22) but recent theoretical1,2 and experimental investigations3,4 have given a boost to this field. Spin current-based electronics with low-energy consumption has since been discussed, where spin-current injection and detection, using charge/spin conversion by direct spin Hall effect and ISHE, played a key role. A variety of materials have subsequently been explored to realize efficient charge/spin conversion5–18. The playground for the exploration was first limited to semiconductors but then extended to metals, where we can take advantage of the less pronounced effect of interfacial barriers. Heavy transition metals such as Pt6–10,14, Au9,12,13, and Pd8,9,11 and also Cu-based alloys17,18 were found to exhibit a particularly large spin Hall angle aSH (the maximum yield of the charge/spin conversion), 0.01–0.1 at room temperature, owing to their pronounced SOC effects. These effects give these metals an advantage for application as a spin injector. In addition to the large aSH, their low electrical resistivity (rC), typically rC ¼ 10 7–10 5 O cm, allows large charge currents to be passed and hence to inject a large spin current without serious Joule heating. Spin currents can be detected by using the ISHE. In contrast to the case for spin injectors, the low rC of the heavy metals with a large aSH is a disadvantages when it comes to spin detection. In the ISHE, the electric voltage DVISHE generated by a spin current IS is in proportion to rC (refs 23,24): DVISHE / aSH rC IS rSH IS :
ð1Þ
Spin Hall resistivity given by rSH aSH rC determines the efficiency of spin-current detection. This means that a sensitive detection of spin current could be achieved in materials with both a large aSH and a high rC. In typical heavy metals, their low rC imposes strong constraints in tuning the value of rSH as it remains as low as o1 mO cm. One of the obvious approaches to improve the performance of spin detectors could be to increase the rC by alloying. Alloying can in fact increase not only the rC but also the aSH through an extrinsic spin Hall effect25–27. At room temperature where the inelastic scattering of charge carriers is dominant, however, it should be hard to anticipate a drastic increase of rC by alloying, for example, more than an order of magnitude increase as compared with the pristine material. Therefore, the improvement of rSH would not be achieved only by alloying. In this work, we propose 5d transition metal oxides (TMOs) as alternative metals to realize both large aSH and large rC, which should enhance rSH. The uniqueness of 5d TMOs is characterized by the extremely strong SOCB0.5–1 eV originating from the predominant 5d character of the conduction band. The SOC in 5d TMOs is in fact as strong as to reconstruct the electronic structures drastically, as first discussed in the case of Jeff ¼ 1/2 Mott state Sr2IrO4 (ref. 28). The analogous predominant SOC effect has been commonly observed in a broad range of Ir oxides including Ba2IrO4 (ref. 29), CaIrO3 (ref. 30) and Ir2O4 (ref. 31). In those Ir oxides, in addition to the strong SOC, the localized character of d orbitals gives rise to a moderately high charge resistivity rC even in the metallic state. Typical rC values of conductive 5d Ir TMOs such as IrO2 and SrIrO3 at room temperature are of the order of 10 4–10 3 O cm, at least one order of magnitude higher than those of normal s metals. As the variety of materials continues to grow rapidly, 5d TMOs offer a 2
unique opportunity to explore the giant rSH for efficient spin detection. We selected a simple binary oxide, rutile IrO2 (refs 32–34), as the basis for our exploration. IrO2 with Ir4 þ shares the same 5d5 configuration with many other Ir oxides, where the strong SOC dominates the electronic states and the resultant electronic properties34. This binary oxide has been long used as an electrode in various device applications, ranging from non-volatile ferroelectric memories to electrochemical devices. The excellent electrode properties are due to the formation of a clean, well-defined interface with other materials owing to its high chemical and thermal stability, and superior barrier properties for oxygen diffusion. In such a clean interface, it may be possible to inject a spin current through a diffusion process; IrO2 is therefore an ideal platform for testing the ISHE of 5d TMOs. Here, we describe successful spin-current injection into IrO2 using a lateral spin-valve (LSV) device geometry and demonstrate the ISHE with a remarkably high rSH as a metal not only in the polycrystalline state but also in the practically important amorphous state. Results Device structure. We fabricated cross-junction-type devices consisting of an IrO2 wire and a permalloy(Ni80Fe20, Py)/Ag/Py LSV35, shown in Fig. 1a,b (see also Methods). Spin currents are passed in the Ag strip by a non-local charge current injection (IC) from the ferromagnetic Py electrode and are perpendicularly injected in part into the IrO2 wire through the diffusion (Fig. 1a). This effect, called spin absorption, enables us to conduct a quantitative analysis of the ISHE as have been demonstrated for various materials7,8,17,18. We examined the potential of polycrystalline and amorphous IrO2 wires as the spin detector element. Their resistivities were 2.0 10 4 O cm and 5.7 10 4 O cm at 300 K, respectively, which are 1–2 orders of magnitude higher than those of metals that have been studied to date as a spin Hall material.
H
V
IC Ag Py1 Py2
IrO2
IrO2 Py1
Py2
Ag
Figure 1 | Inverse spin Hall effect measurements using a spin absorption effect in a lateral spin-valve geometry. (a) The structure of device used for ISHE measurements is shown schematically. A LSV with two Py electrodes (Py1: spin source, Py2: spin detector) bridged by an Ag spin transport layer was formed on an IrO2 wire. Spin-polarized charge current, IC, was injected along the arrow to accumulate pure spin currents in the Ag. The diffusion of spin current into the IrO2 wire, namely, the spin absorption, gives rise to the ISHE in IrO2. (b) Scanning electron microscopy image of a typical device. Scale bar, 500 nm. The dotted lines indicate the side edges of the IrO2 wire for clarity.
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To check that the Ag layer is not oxidized by directly contacting with IrO2, we first characterized the Ag/IrO2 interface by means of interface resistance measurements36. The current– voltage characteristics of the Ag/IrO2 interface showed an ohmic behaviour, typical of metal/metal interface. The slope of the data yielded a resistance–area product (RA) of 2.3 fO m2 at 300 K, which is as low as that of the metallic, transparent Ag/Py interface (RA ¼ 1.9 fO m2 at 300 K). An estimate of the thickness of the possibly oxidized Ag layer, using the resistivities of Ag2O and AgO in the literature37, never exceeded 0.1 nm. These observations imply that the Ag/IrO2 interface in the present devices is very sharp as in metal/metal interfaces. Spin-current injection into IrO2. The spin absorption by IrO2 across the interface was then confirmed by non-local spin-valve (NLSV) experiments7,8,17,18,35. The schematic diagram of the measurement is shown in Fig. 2a. The pure spin currents accumulated in the Ag strip by injecting spin-polarized charge currents IC from Py1 to Ag is detected as a voltage VS ( ¼ V þ V ) between Py2 (V þ ) and Ag (V ) (upper panel). The spin accumulation signal DRS is given by the difference in VS/ IC (RS) between parallel (high RS) and antiparallel (low RS) magnetizations of the two Py wires. If an IrO2 middle wire is in contact with the Ag, the accumulated spin diffuses in part into it (lower panel), resulting in the reduction in DRS (ref. 7). Figure 2b and c show field dependences of RS at 300 and 10 K, respectively. The decrease of DRS by the insertion of the IrO2 middle wire indicates the spin absorption effect. This is more clearly demonstrated in the temperature (T) dependence of DRS with (DRwith ) and without (DRwithout ) the middle wire, as S S is displayed in Fig. 2d. At all the temperatures, DRwith S , while both are enhanced systematically smaller than DRwithout S
at low temperatures owing to the increase of the spin-diffusion length of Ag (lAg)35. By analysing the data based on the threedimensional spin-diffusion model18 (see Supplementary Methods and Supplementary Fig. S1), we estimated a spin-diffusion length in polycrystalline IrO2, lIrO2 ¼ 3.8 nm at 300 K and 8.4 nm at 10 K, which are comparable to those of Pt (3–10 nm at 300 K (refs 6–10,14)) and CuIr (5–20 nm at 10 K (ref. 17)) where relatively large spin Hall angles were observed. This indicates that spin scattering of IrO2 is indeed very strong as expected from the 5d conduction band34. ISHE and qSH of IrO2. By injecting spin currents through the spin absorption effect, we successfully observed ISHE in IrO2. In Fig. 3a,b, we plot the room-temperature ISHE signal RISHE (DVISHE/IC) for polycrystalline and amorphous samples as a function of the magnetic field (The temperature dependence of the ISHE is shown in Supplementary Fig. S2 and is explained in Supplementary Note 1). Here the magnetic field was applied along the hard axis of the Py spin source (see Fig. 1a), and DVISHE was induced along the long-axis direction of the IrO2 wire. Reflecting the magnetization process in hard axis of Py, RISHE linearly increased up to B1,500 Oe and then saturated. The antisymmetric response to the applied magnetic field excludes any spurious effects such as anisotropic magnetoresistance of Py; the ISHE of IrO2 is responsible for the resistance change (2DRISHE) between positive and negative magnetic fields. The in-plane angular dependence of magnetic field effect on RISHE was confirmed fully consistent with the ISHE origin. Figure 3c shows the variation in RISHE under a magnetic field direction rotated by f with respect to the ordinary set-up (Fig. 3d, inset). The sign change of RISHE occurs between f ¼ 0 and p by magnetization switching of Py and concomitant polarization reversal of the spin
Without IrO2
RS (mΩ)
0
VS
H
V
IC
–0.2 –0.4 –0.6
Ag
Py2 With IrO2 H
300 K 10 K
0
RS (mΩ)
Py1
w/o IrO2 w/IrO2
–0.5 –1.0 –1.5
VS V
–2.0 –400 –200 0 200 400 H (Oe)
IC
IrO2
ΔRS (mΩ)
1.5 w/o IrO2
1.0 0.5 w/IrO2 0 0
100 200 T (K)
300
Figure 2 | Non-local spin-valve measurements. (a) The set-up of measurement is schematically depicted. The magnetic field H is applied along the easy axis of the Py electrodes. (b,c) NLSV signals measured at 300 K and 10 K for Py/Ag/Py LSVs without and with the polycrystalline IrO2 middle wire. (d) Temperature dependences of the NLSV signals. NATURE COMMUNICATIONS | 4:2893 | DOI: 10.1038/ncomms3893 | www.nature.com/naturecommunications
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IrO2 Polycrystalline w = 170 nm
RISHE (mΩ)
RISHE (mΩ)
0.2 0.1
2ΔRISHE
0
=0
0 =π
–0.2 –4,000
–0.1
0 H (Oe)
4,000
0.2
2ΔRISHE (mΩ)
RISHE (mΩ)
0.1
Amorphous w = 100 nm w = 170 nm
0
0.1 0 H
–0.1
–0.1
–0.2 –4,000 –2,000
0 H (Oe)
2,000
4,000
0
π/2 (rad)
π
Figure 3 | Inverse spin Hall effect of IrO2 at 300 K. (a) The ISHE signal RISHE (DVISHE/IC) for a polycrystalline IrO2 wire with a width w of 170 nm was measured as a function of the applied magnetic field H. (b) The results for amorphous IrO2 samples. Two devices with different w values (100 and 170 nm) were measured. The 100 nm-width device showed larger RISHE because of the increase of spin-current density. RISHE of the two amorphous devices are smaller than that of the polycrystalline sample shown in a. (c,d) Angular dependence of RISHE and the resistance change 2DRISHE by the ISHE. The in-plane azimuthal angle f with respect to the long axis of Ag is rotated to change the polarization direction of the spin current (inset in d). The solid line in d is a cos f curve fitted to the results.
current. As shown in Fig. 3d, the resistance change 2DRISHE vanishes at f ¼ p/2 and exhibits a cos f relation. This characteristic angular dependence is the hallmark of ISHE7,12, evidencing spin-dependent electron scattering in IrO2. Because of the large difference in rC between Ag and IrO2, the charge current induced in the IrO2 wire by the ISHE is partially shunted by the adjacent Ag layer. To take into account such geometric effects and to precisely determine rSH, we adopted the three-dimensional spin-diffusion model (see also Supplementary Methods). Using the ISHE signal 2DRISHE and data obtained from the NLSV measurements, aSH and rSH are, respectively, calculated to be 0.040 and 8.0 mO cm for polycrystalline IrO2, and 0.065 and 37.5 mO cm for amorphous IrO2 at 300 K. Figure 4 summarizes spin Hall resistivity rSH and electrical resistivity rC for a variety of metals with a large spin Hall angle aSH reported so far, together with that for IrO2. It mimics the point of this work in that rSH of IrO2 is distinctly large compared with typical heavy metals and their alloys of which rSH is B0.16–1.2 mO cm (refs 6–14,17,18), and is now comparable to the large rSH that was recently discovered in ultrathin films of b-phase (A15 crystal structure) W (ref. 15) and Ta (ref. 16). Discussion To generate a large electric voltage using the ISHE of IrO2 from existing metal-based spin-current devices, it is important to reduce the shunting effect at the Ag/IrO2 interface due to their large difference in rC. One of the promising approaches is to use Al (ref. 38) and Mg (ref. 39) as the non-magnetic spin transport layer. Their rC values are one order of magnitude higher than that of Ag we used, of the order of 10 mO cm at room temperature, while a comparably long spin-diffusion length is obtained. Another interesting route is a spin transport layer based on a conductive oxide composed of light elements with small 4
SOC. For example, in ZnO (ref. 40), doping with Al yields rC of the order of 100 mO cm (ref. 41), which can match with that of IrO2. The high chemical stability of IrO2 could be advantageous in fabricating such oxide-based junctions. The discovery of the ISHE in amorphous IrO2, which can be grown at room temperature, is a significant step towards spintronics devices based on such oxide materials. The comparably large aSH in the amorphous form may point to that spin scattering in this compound occurs at the length scale of as short as a unit cell, potentially enabling the spin detection at the atomic layer thickness. Although the physics of spin scattering in amorphous states has not been understood yet, the availability of the amorphous form should make it easier to study SOC-induced transport phenomena in 5d TMOs not used before in spintronics. In conclusion, 5d TMOs are the most promising materials for spin detection in spintronics. We demonstrated that the combination of strong SOC and a moderately high rC is a key to improve the performance of spin detection. These achievements in the simple binary oxide manifest the potential of 5d TMOs as a new class of spintronic materials. Strong SOC in this class of materials produces a rich variety of intriguing physical properties, including correlated topological insulator42, Weyl semi-metal43 and Kitaev spin liquid44. Our discovery of the large spin Hall resistivity may make 5d TMOs even more fascinating. Methods Device fabrication. The Py/Ag/Py LSV with an IrO2 middle wire was fabricated on a SiO2/Si substrate. Au/Ti leads for electrical measurements were prepared on the substrate by a photolithography and an e-beam deposition. IrO2 film was grown by a reactive sputtering with a 99.9% pure Ir target. A wire structure of IrO2 was formed using a posi-type resist patterned by an e-beam lithography. The typical wire width and thickness were 170 and 15 nm, respectively. During the deposition, the substrate was not heated, and the pressure was fixed at 0.7 Pa of Ar/O2 (90:10) mixture gas. X-ray diffraction analysis indicated that the as-deposited IrO2 film was amorphous. The amorphous film turned into
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V 10–4 -W15
a-IrO2
|SH| (Ω cm)
-Ta16 poly-IrO2
10–5
Pt14 CuIr17
CuBi18 10–6
Pt10 Pt9 Pd8
Au12 Pt8 SH=0.1 10–7 –6 10
10–5
Ta8 Nb8 Pd11 Mo8
SH=0.01 10–4 C (Ω cm)
10–3
Figure 4 | Spin Hall resistivity of metals. Experimentally measured values of spin Hall resistivity rSH for various metals are plotted as a function of electrical resistivity rC. Data include Pt (refs 9,10) and Pd (ref. 11) evaluated at room temperature by spin pumping, Pt (ref. 14) and atomic layer thin films of b-W (ref. 15) and b-Ta (ref. 16) at room temperature by spintransfer-torque ferromagnetic resonance, Au at 295 K using a planar Hall device12, Ta, Nb, Pd, Mo, Pt (ref. 8), 12% Ir-doped Cu (ref. 17), 0.5% Bidoped Cu (ref. 18) at 10 K, and polycrystalline and amorphous IrO2 at 300 K (this work) by spin absorption.
polycrystalline after a post-annealing at 400 °C in air. The LSV with a Py–Py separation of 700 nm (centre-to-centre) was then formed onto the IrO2 wire by the shadow evaporation method35,36. To prevent the surface oxidation of Ag, a 2-nmthick MgO protection layer was e-beam deposited on the surface without breaking vacuum. The width and thickness of wire were 170 and 100 nm for Ag, and 170 and 20 nm for Py, respectively. Their rC and spin-diffusion length were 3.0 mO cm and 330 nm for Ag and 47 mO cm and 5 nm for Py, respectively, at 300 K. One of the two Py electrodes was made longer than the other (not shown in Fig. 1b) to make the contrast in the fields for magnetization reversal. Electrical measurements. All electrical measurements were performed by a standard lock-in technique in a He flow cryostat. An alternating current IC of 200 mA with a frequency of 79 Hz was used for NLSV measurements. In ISHE measurements, IC of 400 mA was applied. We confirmed the linearity between the output voltage DVISHE and IC in the range of 100–400 mA.
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Acknowledgements
Additional information
We thank K. Ohgushi for helpful discussions. This work was supported by Grants-in-Aid (number 22340108, 23103518 and 24224010) from MEXT, Japan.
Supplementary Information accompanies this paper at http://www.nature.com/ naturecommunications Competing financial interests: The authors declare no competing financial interests.
Author contributions K.F., Y.F. and J.M. designed the experiments. K.F., Y.F. and H.I. fabricated devices and collected the data. K.F. and Y.N. analysed the data. K.F. wrote the manuscript with input from J.M. Y.O., and H.T. H.T. and Y.O. planned and supervised the project. All authors discussed the results.
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